ACS Applied Energy Materials
·
2021
·
IF 6.024
Peng Zeng,Hao Yu,Hong Liu,Yongfang Li,Ziyi Zhou,Xi Zhou,Changmeng Guo,Bin Li,Manfang Chen,Zhigao Luo,Ying Wang,Baobao Chang,Xianyou Wang
The application of Li-S batteries is hampered by some unresolved issues, including the severe polysulfides shuttle effects and sluggish reaction kinetics. Hence, we designed and prepared tin oxide hydroxide quantum dots (TOH) anchored on a honeycomb porous carbon (HPC) matrix as multifunctional sulfur hosts, and deeply studied the enhancement of TOH on the reaction kinetics of Li-S battery referred to as the apparent activation energy, Li+ ion diffusion coefficient, and reaction barrier. It is proved by density functional theory that the HPC@TOH hosts have a higher binding energy to polysulfides than the simplex carbon matrix. Meanwhile, the catalytic TOH can decrease the surface active energy of the redox reaction and accelerate the conversion of sulfur-containing species. Consequently, by means of the synergistic effects of physical capture and chemical adsorption together with catalytic conversion, the comprehensive performances of Li-S batteries are distinctly promoted. In particular, a Li-S battery using HPC@TOH as a host delivers a good reversible specific capacity of 1342.95 mAh g–1 at 0.1 C. Moreover, with the current increased to 1 C, it shows a relatively satisfactory specific capacity of 918.05 mAh g–1. After 400 cycles, a competitive specific capacity of 688.54 mAh g–1 can still be maintained with a very low fading rate of 0.06% per cycle. Most importantly, when the sulfur areal loading reaches as high as 4.25 mg cm–2 and electrolyte/sulfur ratio is controlled to be as low as 7 μL mg–1, and the Li-S battery using HPC @TOH as a host can still cycle steadily more than 50 cycles at 0.2 C. Therefore, this work provides an effective manner to boost the comprehensive performance of Li-S batteries by virtue of optimizing and designing the host material with synergistic effects of physical capture, chemical adsorption, and catalytic conversion.
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高影响因子
Materials
·
2023
·Vol. 17
·期 1
·6
·
IF 3.4
Yu Lei,Hongdian Chen,Chenyang Shu,Changguo Chen
Developing catalysts with superior activity to hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is equally important to the overall photoelectrochemical water splitting to produce hydrogen. In this work, bismuth oxyiodide (BiOI), iron-modified bismuth iodide Fe/BiOI, and the sulfurized S-Fe/BiOI were prepared using the solvothermal method. The three materials all have good absorption ability for visible light. The photoelectrochemical catalytic activity of BiOI to oxygen evolution reaction (OER) is significantly enhanced after iron modification, while the sulfurized product S-Fe/BiOI exhibits better catalytic activity to hydrogen evolution reaction (HER). Hence, OER and HER can be simultaneously catalyzed by using Fe/BiOI and S-Fe/BiOI as anodic and cathodic catalysts to facilitate the overall photoelectrochemical water splitting process.Keywords:bismuth oxyiodide;iron modification;sulfurization;overall water splitting;photoelectrochemical catalysis
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yuxia Liu,Shiting Wang,Zhifeng Dai,Yubing Xiong
The cycloaddition reaction of CO2 and epoxides to form cyclic carbonates is a promising strategy to alleviate the climate change caused by CO2 in view of its high atomic economic efficiency and solvent-free and mild conditions. Inspired by the mechanism of cycloaddition reactions catalyzed by Lewis acid/Lewis base binary systems, we explored a series of heterogeneous catalysts functionalized by cobalt porphyrin cross-linked phosphonium salt poly(ionic liquid)s. Specifically, poly(4-vinylbenzyl chloride) (PVBnCl) was used as the polymer backbone. Then, PVBnCl was cross-linked by 5,10,15,20-tetra(4-pyridyl) porphyrin (TPyP) and quaternized by triphenylphosphine (PPh3). After complexing with CoCl2 and anion exchange, the as-prepared polymers CoTPyP-c-PVBnPPh3X were characterized using FTIR, SEM, TEM, XPS, TGA, ICP, and solid-state 13C NMR measurements. The results demonstrated that CoTPyP-c-PVBnPPh3X were efficient catalysts for the cycloaddition of CO2 and epoxides under mild conditions. Almost quantitative conversion of epoxides could be achieved at 80 °C and 1 atm CO2, and CoTPyP-c-PVBnPPh3X could be easily separated and reused for four cycles only with a little decrease in the catalysis activity. The synergistic catalysis of the Lewis acid metal center and nucleophilic halogen ion addressed the excellent performance of CoTPyP-c-PVBnPPh3X. Therefore, our findings provided a new solution for the development of efficient heterogeneous catalysts with multi-centers for CO2 conversion.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Li Gong,Xiaojiang Qiu,Dong Cheng,Yao Hu,Zaizhi Zhang,Qunsen Yuan,Dezhi Yang,Chengshuai Liu,Liyuan Liang,Feng He
Sulfidated zero-valent iron (S-ZVI) enhances the degradation of chlorinated hydrocarbon (CHC) in contaminated groundwater. Despite numerous studies of S-ZVI, a versatile strategy to improve its dechlorination kinetics, electron efficiency (εe), and dechlorination capacity is still needed. Here, we used heteroatom incorporation of N(C) and S by ball-milling of microscale ZVI with melamine and sulfur via nitridation and sulfidation to synthesize S-N(C)-mZVIbm particles that contain reactive Fe-NX(C) and FeS species. Sulfidation and nitridation synergistically increased the trichloroethene (TCE) dechlorination rate, with reaction constants kSA of 2.98 × 10–2 L·h–1·m–2 by S-N(C)-mZVIbm, compared to 1.77 × 10–3 and 8.15 × 10–5 L·h–1·m–2 by S-mZVIbm and N(C)-mZVIbm, respectively. Data show that sulfidation suppressed the reductive dissociation of N(C) from S-N(C)-mZVIbm, which stabilized the reactive Fe-NX(C) and reserved electrons for TCE dechlorination. In addition to lowering H2 production, S-N(C)-mZVIbm dechlorinated TCE to less reduced products (e.g., acetylene), contributing to the material’s higher εe and dechlorination capacity. This synergistic effect on TCE degradation can be extended to other recalcitrant CHCs (e.g., chloroform) in both deionized and groundwater. This multiheteroatom incorporation approach to optimize ZVI for groundwater remediation provides a basis for further advances in reactive material synthesis.
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PubMed
高影响因子
JOURNAL OF CONTROLLED RELEASE
·
2024
·
IF 10.5
Tao Bo,Chenfei Wang,Dingjin Yao,Qiuyu Jiang,Yitong Zhao,Feifei Wang,Wei He,Weiyi Xu,Hao Zhou,Ming Li,Si Zhang,Ruyi Xue
Gene delivery to macrophages holds great promise for cancer immunotherapy. However, traditional gene delivery methods exhibit low transfection efficiency in macrophages. The star -shaped topological structure of polymers is known to encapsulate genes inside their cores, thereby facilitating sustained release of the genetic material. Herein, combining the structural advantages of star polymers and the transfection advantages of poly (β-amino ester)s (PAEs), we developed a novel linear oligomer grafting-onto strategy to synthesize a library of multi-terminal star structured PAEs (SPAEs), and evaluated their gene delivery efficiency in various tissue cells. The transfection with human hepatocellular carcinoma cells (HepG2, HCC-LM3 cells and MHCC-97H cells), rat normal liver cells (BRL-3 A cells), human ovarian cancer cells (A2780 cells), African green monkey kidney cells (Vero cells), human cervical cancer cells (HeLa cells), human chondrosarcoma cells (SW1353 cells), and difficult-to-transfect human epidermal keratinocytes (HaCaT cells) and normal human fibroblast cells (NHF cells) showed that SPAEs exhibited superior transfection profile. The GFP transfection efficiency of top-performing SPAEs in HeLa cells (96.1%) was 2.1-fold, and 3.2-fold higher compared to jetPEI and Lipo3000, respectively, indicating that the star-shaped topological structure can significantly enhance the transfection efficiency of PAEs. More importantly, the top-performing SPAEs could efficiently deliver Nod2 DNA to difficult-to-transfect RAW264.7 macrophages, with a high transfection efficiency of 33.9%, which could promote macrophage M1 polarization and enhanced CD8+ T cell response in co-incubation experiments. This work advances gene therapy by targeting difficult-to-transfect macrophages and remodeling the tumor immune microenvironment.
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高影响因子
Heliyon
·
2023
·Vol. 9
·期 7
·e18046
·
IF 4
Weijie Zhang,Lei Shi,Wei Zhou,Xin Liu,Yuan Xi,Xinyin Wang,Ya Li,Xia Xu,Youcai Tang
Breast cancer is one of the most common cancers. Oridonin, a traditional Chinese medicine, is believed to inhibit tumor growth, but its particular effects on breast cancer remain unknown. In this study, we examined oridonin's effects on 4T1, MCF-7, and MDAMB-231 cellular activity using CCK8. Scratch assays were used to detect oridonin's effects on cellular migration. Oridonin's effects on the breast cancer cell cycle were studied using flow cytometry, and expression of cell cycle related proteins p53, CDK2, and p21 was detected using Western blot assays. Metabolomics assays were used to detect changes in small molecule metabolites and metabolic pathways in breast cancer cells after treatment with oridonin. Oridonin's effects on breast cancer growth were also studied using xenograft mice. Metabolomics assays were used to detect changes in metabolites and metabolic pathways in xenograft mouse plasma in a control group, model group, and drug administration group. Experimental results showed that oridonin could significantly inhibit breast cancer growth both in vivo and in vitro. Scratch experiments showed that oridonin could inhibit breast cancer cell migration. Oridonin was also able to arrest cells in S phase by affecting several cell cycle-related proteins, including p53, CDK2, and p21. Metabolomic analysis of 4T1 cells identified a total of 33 differential metabolites, including multiple amino acids (such as l-Glutamic acid, l-Asparagine, l-Histidine, l-Valine, and l-Isoleucine). KEGG pathway enrichment analysis showed significant changes in aminoacyl-tRNA biosynthesis, and in multiple amino acid metabolic pathways. Plasma metabolomic analyses of xenograft mice revealed 28 differentially-expressed metabolites between the different animal model groups, including multiple amino acids. KEGG pathway analysis showed significant alterations in multiple amino acid metabolic pathways in oridonin-treated mice. Additionally, changes in the expression of PI3K, AKT and mTOR proteins, as well as in branched amino acids, suggest that oridonin affects the PI3K/AKT/mTOR signaling pathway by inhibiting the biosynthesis of valine, leucine and isoleucine. Taken together, our results suggest that oridonin has strong anti-tumor activity in vitro and in vivo, and has potential as an adjuvant to breast cancer treatment regimens.
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DOI
PubMed
高影响因子
Polymer Chemistry
·
2016
·Vol. 7
·期 18
·3172-3178
·
IF 5.687
Zikun Wang,Youhua Tao,Zhen Wang,Jingling Yan
Four N-vinyl-1,2,3-triazole monomers were prepared in high yields from 2-aminoethanol and α-diazo-β-oxoamides via modified Wolff's cyclocondensation reactions. Then a series of poly(N-vinyl-1,2,3-triazole)s were synthesized through conventional free radical polymerization of these monomers. The chemical structures of these monomers and polymers were confirmed by proton and carbon nuclear magnetic resonance (1H and 13C NMR). The properties of poly(N-vinyl-1,2,3-triazole)s were systematically characterized by a variety of analytical techniques including thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), gel permeation chromatography (GPC), and solubility testing. The results indicated that these polymers exhibited higher glass transition temperatures (196–212 °C) than most of the commodity vinyl polymers such as polystyrene (100 °C) and poly(methyl methacrylate) (110 °C). Moreover, these polymers can be further functionalized through hydrolysis of amide groups. These results revealed that this methodology has great potential for constructing 1,2,3-triazole-containing monomers and polymers.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 2
·114
·
IF 3.444
Ke Yu,Yan Lin,Jinchen Fan,Qiaoxia Li,Penghui Shi,Qunjie Xu,Yulin Min
Ethanol oxidation reaction (EOR) is an important electrode reaction in ethanol fuel cells. However, there are many problems with commercial ethanol oxidation electrocatalysts today, such as poor durability, poor anti-CO poisoning ability, and low selectivity for C–C bond cleavage. Therefore, it is very meaningful to develop a high-performance EOR catalyst. Herein, we designed ternary N, S, and P-doped hollow carbon spheres (C–N,P,S) from polyphosphazene (PCCP) as Pd supports for EOR. Using SiO2spheres as the templates, the PCCP was first coated on the surfaces of SiO2spheres by in situ polymerization. Through high-temperature pyrolysis and hydrofluoric acid-etching, the hollow PCCP has a large surface area and porous structure. After loading Pd nanoparticles (NPs), the Pd/C–N, P, S catalysts with Pd NPs decorated on the surfaces of C–N, P, S can achieve a high mass peak current density of 1686 mA mgPd−1, which was 2.8 times greater than that of Pd/C. Meanwhile, the Pd/C–N, P, S catalyst also shows a better stability than that of Pd/C after a durability test of 3600s.
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高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 42
·22584-22591
·
IF 14.511
Xiaoying Song,Min Wang,Sheng Wang,Zhu Cheng,Ting Zhang,Ting Zhu,Hucheng Song,Linwei Yu,Jun Xu,Kunji Chen
Solid-sate lithium-ion batteries (LIBs), especially lithium–sulfur (Li–S) batteries, are one of the most promising candidates for developing high energy density and high safety energy storage devices. However, current solid-state Li–S batteries can only work well at a relatively high operating temperature (>50 °C) due to the poor Li-ion transfer kinetics at electrodes/electrolyte and their interfaces which make these batteries lose most of their capacity and power as the temperature falls below room temperature. Here, we report an extra-wide operating temperature solid-state Li–S battery that can efficiently harvest omnidirectional solar energy and convert it into heat via a hierarchical copper–silicon nanowire photothermal current collector. Such a current collector enables broad solar spectrum absorption (>93%) with a wide incident angle (0 degree to 70 degree) and efficient conversion of light-to-heat, improving charge storage and transmission at electrodes/electrolyte and their interfaces even at low operating temperatures. As a result, the battery demonstrates low impedance (∼102 Ω cm2), a high discharge capacity of ∼900 mA h g−1 at room temperature, ∼960 mA h g−1 at 60 °C and a discharge capacity of ∼260 mA h g−1 at −60 °C. Such a design provides an effective solution for all-solid-state LIBs operating at a low temperature.
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高影响因子
RSC Advances
·
2018
·Vol. 8
·期 8
·4119-4124
·
IF 2.936
Pengpeng Zhang,Qing Yu,Xue Min,Linbao Guo,Jiangjian Shi,Xiangyun Zhao,Dongmei Li,Yanhong Luo,Huijue Wu,Qingbo Meng,Sixin Wu
The annealing temperature of solution-processed Cu2ZnSn(S,Se)4 (CZTSSe) precursor films has been carefully optimized for favorable selenization. At higher temperature, more solvent will be removed, and the crystallinity of the precursor films can be improved. It is found that, although the crystallinity of selenized film is continuously enhanced by increasing the temperature, a dense CZTSSe film with round and large grains can only be achieved at medium high temperature ranging from 350 to 400 °C. Further investigation reveals that, in this regime, the carrier and defect densities are obviously reduced, leading to average photoelectric conversion efficiency (PCE) improved from 5.1% to 9.4%. An optimal annealing temperature of 380 °C is obtained and up to 10.04% of photoelectric conversion efficiency has been achieved.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Ziyu Qin,Xiaoxiao Song,Junyong Wang,Xiang Li,Congyi Wu,Xiaoxia Wang,Xueqiong Yin,Dawen Zeng
For the important applications of gas identification related to specific diseases in healthcare, flexible gas sensors have attracted more attention. Among them, two-dimensional transition metal dichalcogenides (2D TMDs) have been known as good promising flexible gas-sensitive materials. While how to tightly attach 2D materials on flexible substrates is still challenging. Here, we propose an enhanced room-temperature flexible paper-substrate sensors based on 2D tungsten disulfide (WS 2 ) with S defects, which are facilely synthesized by chemical exfoliation and vacuum filtration method. Structure characterization shows that most of the as-prepared 2D WS 2 are within 3 layers. Spectroscopic characterization proves the existence of S defects on the surface of 2D WS 2 produced by chemical exfoliation. The room-temperature (25 °C) NH 3 gas sensitivity results show that the response intensity of 2D WS 2 with rich S defects is nearly three times higher than the highly crystalline 2D WS 2 . The results of the flexible gas sensitivity indicate the fast response and high stability of our devices in breathing detection and bending experiments. Furthermore, the devices can effectively distinguish bending stress changes and gas-sensitive response signals at the same time, realizing multifunctional sensing detection. Our work will be a reference for fabricating flexible sensors based on 2D materials.
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高影响因子
Catalysis Science & Technology
·
2012
·Vol. 2
·期 11
·2332-2340
·
IF 0
Jiefeng Hu,Yuping Wang,Min Han,Yaoming Zhou,Xiaoqing Jiang,Peipei Sun
Fe3O4 and Pd nanoparticles were assembled on sulfonated graphene (s-G) by an easy chemical approach and characterized by transmission electron microscopy, X-ray diffraction and energy dispersive X-ray spectroscopy. The resulting material could be dispersed homogeneously in water or water/ethanol and further used as an excellent semi-heterogeneous catalyst for the Suzuki–Miyaura cross-coupling reaction in an environmentally friendly solvent under ligand-free ambient conditions. The high heterogeneous catalytic activity appears to be due to the small size of Pd nanoparticles and homogeneous distribution of the nanoparticles on the Fe3O4/s-G matrix. In addition, the catalytic activity did not deteriorate even after repeated applications, which may be due to the easy and efficient magnetic separation of the catalyst and the high dispersion and stability of the catalyst in an aqueous solution.
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危险品化学品经营许可证（带存储）